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The modified multifunctional electrodes for electro-Fenton (EF) process are suggested to be promising cathodes for in situ electro-generation and activation of H2O2 to produce hydroxyl radicals (•OH). However, heterogeneous EF process still faces the challenges of limited catalytic activity and releasing of massive amounts of transition metals to the solution after removal of organic pollutants. The main aim of the present investigation was to prepare a cathode containing carbon nanotubes (CNTs) and CuFe nano-layered double hydroxide (NL